Modelling the coupled mercury-halogen-ozone cycle in the central Arctic during spring

Author:

Ahmed Shaddy1,Thomas Jennie L.1,Angot Hélène123,Dommergue Aurélien1,Archer Stephen D.4,Bariteau Ludovic56,Beck Ivo2,Benavent Nuria7,Blechschmidt Anne-Marlene8,Blomquist Byron56,Boyer Matthew9,Christensen Jesper H.10,Dahlke Sandro11,Dastoor Ashu12,Helmig Detlev313,Howard Dean356,Jacobi Hans-Werner1,Jokinen Tuija914,Lapere Rémy1,Laurila Tiia9,Quéléver Lauriane L. J.9,Richter Andreas8,Ryjkov Andrei12,Mahajan Anoop S.15,Marelle Louis16,Pfaffhuber Katrine Aspmo17,Posman Kevin4,Rinke Annette11,Saiz-Lopez Alfonso7,Schmale Julia2,Skov Henrik10,Steffen Alexandra18,Stupple Geoff18,Stutz Jochen19,Travnikov Oleg20,Zilker Bianca8

Affiliation:

1. 1Université Grenoble Alpes, CNRS, IRD, Grenoble INP, IGE, Grenoble, France

2. 2Extreme Environments Research Laboratory, Ecole Polytechnique Federale de Lausanne (EPFL) Valais Wallis, Sion, Switzerland

3. 3Institute of Arctic and Alpine Research, University of Colorado, Boulder, CO, USA

4. 4Bigelow Laboratory for Ocean Sciences, East Boothbay, ME, USA

5. 5Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA

6. 6NOAA, Physical Sciences Laboratory, Boulder, CO, USA

7. 7Department of Atmospheric Chemistry and Climate, Institute of Physical Chemistry Rocasolano, CSIC, Madrid, Spain

8. 8Institute of Environmental Physics, University of Bremen, Bremen, Germany

9. 9Institute for Atmospheric and Earth System Research/INAR-Physics, Faculty of Science, University of Helsinki, Helsinki, Finland

10. 10Department of Environmental Science, iClimate, Aarhus University, Roskilde, Denmark

11. 11Alfred Wegener Institute (AWI), Helmholtz Centre for Polar and Marine Research, Potsdam, Germany

12. 12Air Quality Research Division, Environment and Climate Change Canada, Dorval, Quebec, Canada

13. 13Current address: Boulder AIR, Boulder, CO, USA

14. 14Climate and Atmosphere Research Centre (CARE-C), The Cyprus Institute, Nicosia, Cyprus

15. 15Indian Institute of Tropical Meteorology, Ministry of Earth Sciences, Pune, India

16. 16LATMOS/IPSL, Sorbonne Université, UVSQ, CNRS, Paris, France

17. 17NILU–Norwegian Institute for Air Research, Kjeller, Norway

18. 18Environment and Climate Change Canada, Toronto, Ontario, Canada

19. 19Department of Atmospheric and Oceanic Sciences, University of California, Los Angeles, CA, USA

20. 20Meteorology Synthesizing Centre-East, EMEP, Moscow, Russia

Abstract

Near-surface mercury and ozone depletion events occur in the lowest part of the atmosphere during Arctic spring. Mercury depletion is the first step in a process that transforms long-lived elemental mercury to more reactive forms within the Arctic that are deposited to the cryosphere, ocean, and other surfaces, which can ultimately get integrated into the Arctic food web. Depletion of both mercury and ozone occur due to the presence of reactive halogen radicals that are released from snow, ice, and aerosols. In this work, we added a detailed description of the Arctic atmospheric mercury cycle to our recently published version of the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem 4.3.3) that includes Arctic bromine and chlorine chemistry and activation/recycling on snow and aerosols. The major advantage of our modelling approach is the online calculation of bromine concentrations and emission/recycling that is required to simulate the hourly and daily variability of Arctic mercury depletion. We used this model to study coupling between reactive cycling of mercury, ozone, and bromine during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) spring season in 2020 and evaluated results compared to land-based, ship-based, and remote sensing observations. The model predicts that elemental mercury oxidation is driven largely by bromine chemistry and that particulate mercury is the major form of oxidized mercury. The model predicts that the majority (74%) of oxidized mercury deposited to land-based snow is re-emitted to the atmosphere as gaseous elemental mercury, while a minor fraction (4%) of oxidized mercury that is deposited to sea ice is re-emitted during spring. Our work demonstrates that hourly differences in bromine/ozone chemistry in the atmosphere must be considered to capture the springtime Arctic mercury cycle, including its integration into the cryosphere and ocean.

Publisher

University of California Press

Subject

Atmospheric Science,Geology,Geotechnical Engineering and Engineering Geology,Ecology,Environmental Engineering,Oceanography

Reference177 articles.

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2. Ahmed, S, Thomas, JL, Marelle, L.2022Regional-Modeling-LATMOS-IGE/WRF-Chem-Polar: WRF-Chem 4.3.3 including mercury chemistry. Zenodo. DOI: http://dx.doi.org/10.5281/zenodo.7137482.

3. Amos, HM, Jacob, DJ, Holmes, CD, Fisher, JA, Wang, Q, Yantosca, RM, Corbitt, ES, Galarneau, E, Rutter, AP, Gustin, MS, Steffen, A, Schauer, JJ, Graydon, JA, Louis, VLS, Talbot, RW, Edgerton, ES, Zhang, Y, Sunderland, EM.2012. Gas-particle partitioning of atmospheric Hg(II) and its effect on global mercury deposition. Atmospheric Chemistry and Physics12(1): 591–603. DOI: http://dx.doi.org/10.5194/acp-12-591-2012.

4. Angot, H, Archer, S, Bariteau, L, Blomquist, B, Helmig, D, Howard, D, Hueber, J, Jacobi, HW, Posman, K.2022a. Gaseous elemental mercury concentrations measured in the University of Colorado container during the 2019-2020 MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition. Arctic Data Center. DOI: http://dx.doi.org/10.18739/A2C824G3G.

5. Angot, H, Blomquist, B, Howard, D, Archer, S, Bariteau, L, Beck, I, Boyer, M, Crotwell, M, Helmig, D, Hueber, J, Jacobi, HW, Jokinen, T, Kulmala, M, Lan, X, Laurila, T, Madronich, M, Neff, D, Petäjä, T, Posman, K, Quéléver, L, Shupe, MD, Vimont, I, Schmale, J.2022b. Year-round trace gas measurements in the central Arctic during the MOSAiC expedition. Scientific Data9(1): 723. DOI: http://dx.doi.org/10.1038/s41597-022-01769-6.

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